A new manganese(I) N-heterocyclic carbene electrocatalyst containing a benzimidazole-pyrimidine-based ligand is reported for the two-electron conversion of CO. The increased π acidity of pyrimidine shifts the two-electron reduction to -1.77 V vs Fc/Fc, 70 mV more positive than that for MnBr(2,2'-bipyridine)(CO); increased catalytic current enhancement is also observed (5.2× vs 2.1×). Theoretical analyses suggest that this heightened activity may follow from the preference for a reduction-first dehydroxylation mechanism.
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Mn-NHC Electrocatalysts: Increasing π Acidity Lowers the Reduction Potential and Increases the Turnover Frequency for CO Reduction.
Inorg Chem
October 2016
Department of Chemistry and ‡Center for Computational Quantum Chemistry, University of Georgia, Athens, Georgia 30602, United States.
A new manganese(I) N-heterocyclic carbene electrocatalyst containing a benzimidazole-pyrimidine-based ligand is reported for the two-electron conversion of CO. The increased π acidity of pyrimidine shifts the two-electron reduction to -1.77 V vs Fc/Fc, 70 mV more positive than that for MnBr(2,2'-bipyridine)(CO); increased catalytic current enhancement is also observed (5.
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